Journal
NANOSCALE
Volume 6, Issue 21, Pages 12626-12634Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c4nr03625e
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Funding
- NSF EPSCOR (NSF) [EPS1004083]
- NSF BRIGE [EEC 1342185]
- Department of Education for a Graduate Assistance in Areas of National Need (GAANN) Fellowship [P200A090323]
- Directorate For Engineering
- Div Of Engineering Education and Centers [1342185] Funding Source: National Science Foundation
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In this work, we employed wet chemically synthesized bimetallic Au-Ag core-shell nanostructures (Au-AgNSs) to enhance the photocurrent density of mesoporous TiO2 for water splitting and we compared the results with monometallic Au nanoparticles (AuNPs). While Au-AgNSs incorporated photoanodes give rise to 14x enhancement in incident photon to charge carrier efficiency, AuNPs embedded photoanodes result in 6x enhancement. By varying nanoparticle concentration in the photoanodes, we observed similar to 245x less Au-AgNSs are required relative to AuNPs to generate similar photocurrent enhancement for solar fuel conversion. Power-dependent measurements of Au-AgNSs and AuNPs showed a first order dependence to incident light intensity, relative to half-order dependence for TiO2 only photoanodes. This indicated that plasmonic nanostructures enhance charge carriers formed on the surface of the TiO2 which effectively participate in photochemical reactions. Our experiments and simulations suggest the enhanced near-field, far-field, and multipolar resonances of Au-AgNSs facilitating broadband absorption of solar radiation collectively gives rise to their superior performance in water splitting.
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